ChemistrySelect
·
2022
·Vol. 7
·期 45
·e202202260
·
IF 2.307
Minghui Wang,Ting Shu,Xinfeng Ge,Jun Hu,Yunxiao Liang
Graphical The 3D continuous pass-through macroporous channels allow fast mass transfer. Abundant mesopores with short channel remarkably enhance the accessibility of the active sites. The abundant micropores provide large amounts of anchoring sites for Ag NPs loading. The uniformly dispersed and ultrafine Ag NPs (2.04 nm) can transfer the interfacial electrons from BH4 − to 4-NP − more efficiently. Developing easily recyclable noble metal nanoparticle-based heterogeneous catalysts is highly desirable for the practical applications. Herein, a millimeter-sized hierarchical porous titanosilicate (HPTS) was prepared by the multi-template method. Various characterization results reveal that HPTS combines the structural advantages of monolith materials and nanomaterials. HPTS is used as an advanced support to construct the Ag/HPTS catalysts via the Ag + in situ reduction on its pore wall. Ag/HPTS shows high catalytic activity for 4-nitrophenol (4-NP) reduction with the TOF values of 3.91 min −1 , which can be attributed to the ultrafine Ag NPs (2.04 nm) and the unique structure of HPTS. The 3D pass-through macroporous channels facilitate mass transfer. The mesopores with ultra-short channel remarkably enhance the accessibility of the active sites. The abundant mesopores and micropores effectively confine the Ag NPs size. Moreover, Ag/HPTS demonstrated good stability and recyclability.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Jing Jiang,Wei Wei,Ying Tang,Shiyu Yang,Xinzhi Wang,Ying Xu,Lunhong Ai
Catalytic hydrogenation reduction based on sodium borohydride (NaBH4) has gained attention as an appealing “one-stone-two-birds” approach for the simultaneous elimination of nitroaromatic pollutants and the production of high-value aminoaromatics under mild conditions. However, the slow kinetics of NaBH4 dissociation on the surface of catalysts restrict the catalytic hydrogenation reduction efficiency. Herein, we report an intelligent localized sulfidation strategy for an in situ implantation of Bi2S3 nanorods within quasi-Bi-MOF architectures (Bi2S3@quasi-Bi-MOF) by fine-tuning the pyrolysis temperature. In this novel Bi2S3@quasi-Bi-MOF, the porous quasi-Bi-MOF enables efficient adsorption of BH4– and 4-nitrophenol (4-NP), while Bi2S3 facilitates the BH4– dissociation to form Hads* species adsorbed on the catalyst surface. Benefiting from the synergistic structure, Bi2S3@quasi-Bi-MOF exhibits excellent performance for the catalytic reduction of 4-NP, delivering a high turnover frequency (TOF) of 1.67 × 10–4 mmol mg–1 min–1 and an extremely high normalized rate constant (knor) of 435298 s–1 g–1. The kinetic analysis and electrochemical tests indicate that this catalytic hydrogenation reduction follows the Langmuir–Hinshelwood mechanism. This study enriches the synthetic strategy of MOF-based derivatives and offers a new catalytic platform for hydrogenation reduction reactions.
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Journal of the Iranian Chemical Society
·
2023
·Vol. 20
·期 5
·1145-1154
·
IF 2.4
Liu Jun,Lan Lixin,Liu Xuanyan,Zhou Quan,Li Rong
In this paper, Cu x OAu–ZnO nano-catalysts with different morphologies were synthesized by one-step replacement method. The nano-catalysts are characterized by scanning electron microscopy, energy-dispersive X-ray analysis, transmission electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. These novel Cu x OAu–ZnO nano-catalysts exhibit exceptionally high stability and superior 4-nitrophenol to 4-aminophenol hydrogenation ability. The relationship between catalytic performances and changes of composition were investigated, and the catalytic activity decreased in the following order: Cu x O 30 Au 35 –ZnO > Cu x O 38 Au 35 –ZnO > Cu x O 21 Au 45 –ZnO. The influence of catalytic conditions for the performance of catalysts has also studied. For the Cu x O 30 Au 35 –ZnO catalysts, the rate constant k app could be up to 18.6 × 10 −3 s −1 , and the conversion of the 4-NP could still reach 98.66% after five cycles. The high activity of Cu x O 30 Au 35 –ZnO may be attributed to the synergistic effect between Au and Cu element. The unique structure and high catalytic performance make Cu x OAu–ZnO nano-catalysts for practical applications in 4-nitrophenol reduction.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 5
·2006-2017
·
IF 3.442
Zhao Yiming,Guo Yingchun,Wang Xiaomei,Zhang Xu
To construct secondary processes of multiscale architecturing, wrinkly silica microspheres (WSMs) are nested into the empty chamber of templated macroporous structure by using core–shell microspheres to self-assemble the colloidal crystal template and selectively removing the shells. It is a universal approach to form the binary inverse opal (IO) structures and maintain interconnected nanochannels. With gold nanoparticles loaded on the WSMs (denoted Au-WSMs@IO SiO 2 ) in the meantime, it has been demonstrated by the reduction of 4-nitrophenol (4-NP) that the binary IO materials (Au-WSMs@IO SiO 2 ) exhibited higher catalytic efficiency than simple nested microspheres (Au-WSMs) after recycling 15 times. Furthermore, it was nice to see it had excellent catalytic effect in the epoxidation of styrene. Owing to the outstanding catalytic activity, recyclability and mechanical stability of the binary IO materials, it will be a promising way to widely apply in heterogeneous catalysis.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Xiaoqiu Yao,Ming Jin,Jiang Du,Decheng Wan
In the jigsaw puzzle of quality gold nanoclusters (AuNCs), those protected by weak ligands or coligands are still rarely available. Here, we provide an example in the case of supported AuNCs. Branched polyethylenimine (PEI, diameter of 1.86 nm) is introduced as discrete molecular patches onto the support of mesoporous polymer beads. Each patch is derived into polyaminophosphine with 2-(diphenylphosphino) benzaldehyde (dppb). The molecular patch is of nanoscale and uniform size. The polymer beads after PEI loading bear unimodal pores (3.9 nm), and the specific surface area is of 390 m2 g–1. AuNCs are obtained by mildly heating the mixture of the functionalized beads and aqueous chloroauric acids. Uniform AuNCs with a diameter of 1.2 ± 0.2 nm (∼53 Au atoms) are obtained when each PEI patch bears 17 dppb ligands, smaller than that of 3.5 nm in the absence of any dppb, suggesting that dppb enhances the nucleation of AuNCs. The heteroleptic AuNCs show ultrahigh catalytic performance (TOF = 391 h–1) for the reduction of 4-nitrophenol, where the dppb ligands hardly suppress the catalytic activity. The catalyst is well recoverable and durable for the reduction of 4-nitrophenol.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 24
·10530-10537
·
IF 9.8
Jiangang Yu,Pingnian Bao,Jia Liu,Yi Jin,Jie Li,Yanwen Lv
In this study, cellulose nanofibrils (CNF) and transition metals (Cu and Ni) were used as the matrix and doping agents, respectively, for the controllable synthesis of ZnO@CNF nanocomposites with adjustable visible-light photocatalytic properties. All samples were elaborately characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller, X-ray diffraction, scanning electron microscopy-energy dispersive spectrometry, X-ray photoelectron spectroscopy, UV-Vis diffuse reflectance and photocurrent response. Several nano-ZnO particle morphologies, including plate, nanorod, sphere, and star, were produced and anchored on the CNFs by controlling the ZnO loading ratio. The as-produced ZnO@CNF nanocomposites exhibited a remarkable photocatalytic degradation of methyl orange under visible-light irradiation. The plate-like ZnO0.6@CNF exhibited the best photodegradation efficiency (53.1%) for methyl orange under blue light (λmax = 450 nm, 50 W) irradiation. Furthermore, when doped with transition metals, Cu or/and Ni–ZnO0.6@CNF exhibited better photocatalytic efficiency than pristine ZnO0.6@CNF. Under blue light irradiation, the preferred Cu/Ni–ZnO0.6@CNF nanocomposite sample demonstrated an enhanced degradation efficiency for various wastewater pollutants, including methyl orange (96.6%), tetracycline hydrochloride (96.6%), rhodamine B (99.0%), 4-nitrophenol (94.7%), bromocresol green (92.9%), bromothymol blue (88.3%), methylene blue (87.7%), 2-chlorophenol (27.5%), and aniline (19.5%), with the recyclability of more than ten times. This study provides new insights into the regulation of ZnO morphology for synthesizing efficient ZnO@CNF photocatalysts for wastewater pollutant degradation under visible-light irradiation.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 47
·17974-17980
·
IF 4
Liqing Li,Xin Deng,Jiani He,Huan Zhang,Li Li,Lihua Zhu
Herein, we report that Pd nanoparticles (NPs) anchored on graphitic nitride carbon (Pd/g-C3N4) catalysts with various Pd contents (1.55 wt%, 0.14 wt%, 0.04 wt%) are successfully prepared via a simple NaBH4 reduction method, exhibiting excellent catalytic activity and selectivity toward 4-aminophenol (4-AP) in 4-nitrophenol (4-NP) selective hydrogenation. 4-NP is completely converted to 4-AP (yield ∼ 100%) under quite moderate reaction conditions (40 °C, 2.0 MPa H2 and 5 min) over the 1.55 wt% Pd/g-C3N4 catalyst, with a high reaction rate r = 134.4 mol4-NP molPd−1 min−1. The excellent catalytic performance can be attributed to the following reasons: (1) a higher ratio of Pd(0)/Pdn+ provides much more exposed active sites for the potential adsorption and activation of the reactants, which is beneficial for increasing the reaction rate and catalytic activity; (2) Pd NPs are highly dispersed on g-C3N4 due to the strong interaction of Pd–N or Pd–C; (3) the interfacial synergism effect between Pd NPs and g-C3N4 enables the effective adsorption and activation of H2 (4-NP) at Pd (g-C3N4), promoting the catalytic hydrogenation of 4-NP and improving their catalytic properties. In addition, this catalyst has superior reusability.
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LANGMUIR
·
2023
·
IF 3.9
Jingyun Ye,Chenhui Li,Xiaoqiu Yao,Ming Jin,Decheng Wan
We here show that a dendritic molecule combined with ligand merit confers supported platinum nanoclusters (PtNCs) with unprecedented catalytic performance. Branched polyethylenimine (PEI, Mn = 2000 D) patched on a porous bead is modified with 2-(diphenylphosphino)benzaldehyde (dppb) before being used to mediate a platinum nanoparticle/nanocluster (Pt0). The catalytic activity of Pt0 toward the reduction of 4-nitrophenol (4-NP) is evaluated from the parameter of Pt-normalized rate constant (kc). Optimization of the dppb level along with transformation of the PEI hydrogens into diol or trimethylammonium groups imparts supported Pt0 unprecedented activity (kc = 19.2 L mmol–1 s–1 and turnover frequency (TOF) = 1041 h–1). The supported Pt0 at an extremely low dosage of 0.1 ppm promotes 98% conversion of 4-NP within minutes and is well recyclable. The striking catalytic activity is attributed to the combination of orthogonal ligand properties such as weak ligand nature, catalyst-activating ability, excellent substrate affinity, and effect on PtNC-size mediation of the ligand.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-15
·
IF 16.6
Wei Shengjie,Sun Yibing,Qiu Yun-Ze,Li Ang,Chiang Ching-Yu,Xiao Hai,Qian Jieshu,Li Yadong
Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N 4 sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N 4 sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N 4 sites.
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Polymers
·
2023
·Vol. 15
·期 23
·4524
·
IF 5
Long Dong,Fajun Zhao,Huili Zhang,Yongjian Liu,Qingyu Huang,Da Liu,Siqi Guo,Fankun Meng
Steam flooding is an effective development method for heavy oil reservoirs, and the steam flooding assisted by the profile control system can plug the dominant channels and further improve the recovery factor. High-temperature-resistant foam as a profile control system is a hot research topic, and the key lies in the optimal design of the foam system. In this paper, lignin was modified by sulfonation to obtain a high-temperature-resistant modified lignin named CRF; the foaming agent CX-5 was confirmed to have good high-temperature foaming ability by reducing the surface tension; the formula of the profile control system (A compound system of CRF and CX-5, abbreviated as PCS) and the best application parameters were optimized by the foam resistance factor. Finally, the effect of PCS-assisted steam flooding in enhanced oil recovery was evaluated by single sand packing tube flooding, three parallel tube flooding, and large-scale sand packing model flooding experiments. The results show that CX-5 has a good high-temperature foaming performance; the foam volume can reach more than 180 mL at 300 °C, and the half-life is more than 300 s. The optimal PCS formulation is 0.3 wt% CRF as an oil displacement agent + 0.5 wt% CX-5 as a foaming agent. The optimal gas–liquid ratio range is 1:2 to 2:1, and the high pressure and permeability are more conducive to the generation and stability of the foam. Compared with steam flooding, PCS-assisted steam flooding can improve oil recovery by 9% and 7.9% at 200 °C and 270 °C, respectively. PCS can effectively improve the heterogeneity of the reservoir, and increase the oil recovery of the three-parallel tube flooding experiment by 28.7%. Finally, the displacement results of the sand-packing model with large dimensions show that PCS can also expand the swept volume of the homogeneous model, but the effect is 9.46% worse than that of the heterogeneous model.Keywords:steam flooding;foam;profile control;enhance oil recovery;high temperature
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiuli Chang,Fengfeng Song,Fang Xu,Dapeng Wu,Yan Hou,Kai Jiang,Yuming Guo,Zhiyong Gao
Charge redistribution across heterointerfaces is an important tactic to enhance the catalytic activities and bifunctionality of hybrid catalysts, especially for green hydrogen production from water electrolysis and harmless electrocatalytic valorization of organics. Herein, a self-supported p-n junction catalytic electrode was constructed by tandem electrodeposition of nickel cobalt phosphide (NiCoP) and nickel iron layered double hydroxide (NiFe LDH) onto Ni foam (NF) substrate, denoted as NiCoP@NiFe LDH/NF, to enhance the electrocatalytic capabilities for water electrolysis and hydrogenation of an organic, para -nitrophenol (4-NP). Benefitting from the charge redistribution across the p-n junction, high electrocatalytic efficiencies for oxygen evolution reaction (OER, overpotential of 388 mV at 100 mA cm −2 ) and hydrogen evolution reaction (HER, overpotential of 132 mV at 10 mA cm −2 ) could be achieved concurrently by the NiCoP@NiFe LDH/NF electrode, and both overpotentials were located within the mainstream levels in this domain. The bifunctional catalytic features enabled a full water electrolysis response of 10 mA cm −2 at 1.61 V. In addition, the p-n junction electrode catalyzed the hydrogenation of 4-NP at a conversion of 100%, para -aminophenol (4-AP) selectivity of 90% and faradaic efficiency (FE) of 88% at −0.18 V. The current work offers a feasible strategy for fulfilling electrochemical H 2 production and hydrogenation valorization of 4-NP pollutant by constructing a self-supported p-n junction catalytic electrode.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiwen Qin,Changkun Ding,Yingying Tian,Jiankang Dong,Bowen Cheng
The uncontrolled release of nitrophenol and dye pollutants into water systems is an increasingly serious worldwide concern, and thus efficient wastewater treatment technologies are urgently needed. Herein we report a novel two-dimensional (2D) transition metal carbides and/or nitrides (Ti3C2Tx MXene) membrane modified with silver nanowires (AgNWs) by vacuum assisted filtration technology for the ultrafast nitrophenol catalysis and water purification applications. Regular and controllable membrane transport channels were constructed by stacking Ti3C2Tx MXene nanosheets. Furthermore, the intercalation of AgNWs into the Ti3C2Tx MXene interlayer greatly enlarged the interlayer spacing, resulting in more gaps for fast and selective molecular transport. The optimized Ti3C2Tx MXene@AgNWs (M@A) membrane exhibited a water flux up to ∼191.9 L/(m2 h) while maintaining a high bovine serum albumin (BSA) rejection of ∼95.4%. We emphatically used M@A membranes as efficient catalysts for the reduction of 4-nitrophenol (4-NP), and the results indicated that M@A-12% membrane exhibited the greatest catalytic reduction ability, and recycling utilization. M@A-12% membrane also had an antibacterial rate of more than 99% against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). This work provides a possibility to expand the application of 2D multifunctional M@A membranes in wastewater treatment and pollutant catalytic degradation.
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